Abstract
ZIF-8 derived carbons demonstrate admirable application prospects in electrocatalytic fields, while ZnNx remaining in those materials are overlooked, crippling the validity of theoretic studies in researches. Herein, the residual Zn in ZIF-8 derived carbons are found could exceed 10 wt% even at carbonization temperatures over 900℃, and Zn-NCs with various Zn contents are adopted as supports to synthesize low-platinum ORR catalysts. Substantial characterizations manifest that ZnNx in Zn-NC can not only provide Zn source for L10-PtZn intermetallic, but act as ‘spatial barriers’ to prevent the formation of inactive PtNx, elevating the active Pt proportion in catalyst by ∼104%. The resultant Zn-NC-Ar-PtZn exhibits a mass activity of 0.557 mA/gPt and a peak density of 1.485 W/cm2. DFT calculations show the strong thermodynamic tendency of forming PtN4 without the protection of ZnN4, and the superior durability and activity of Zn-NC-Ar-PtZn should be attributed to its Zn-derived ligand effects and the SMSI.
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